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Direct synthesis of a disinfectant with fresh scent of green plants by semi-hydrogenation of alkynol on Pd single-atom catalysts

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Nano Research 2024年第5期17卷 3872-3878页

作者： Yan Jiang Xuetong Yu Yuxia Ji Xunzhu Jiang Yalin Guo Tianbo Li Liang Gao Rui Lang Yanxiong Fang botao qiao Jinxiang Dong School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory(Rongjiang Laboratory) Jieyang 515200China CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116024China Guangdong Provincial Key Laboratory of Plant Resources Biorefinery Guangzhou 510006China School of Chemical Engineering and Technology China University of Mining and TechnologyXuzhou 221116China

Alcohol-based disinfectants have protected people in the coronavirus disease 2019(COVID-19)pandemic,but olfactory stimuli of ethanol may evoke unpleasant memories associated with stressful situations in the devastating infectious *** smell of ethanol in household cleaning and disinfectant products can be covered up by the fragrance additives,and 3-hexenol is especially appreciated for the characteristic,strong odor of green *** production of 3-hexenol relies on the selective hydrogenation of 3-hexyn-1-ol,where Lindlar catalyst is normally used for the superior *** achieving such catalytic transformation in ethanol solution seems as a direct way to produce a disinfectant with green aroma,a popular consumer product in the post-COVID era,severe leaching of toxic Pb hinders Lindlar catalyst as a promising *** find that the Fe_(2)O_(3) supported Pd single-atom catalyst is highly selective to fulfill semi-hydrogenation of 3-hexyn-1-ol in 75%ethanol,and the aforementioned household product is readily generated after filtrating the stable,solid catalyst out of reaction ***-atom catalysts have been frequently utilized for fine-chemical synthesis,while in this work they make stunning debut in practical manufacture of daily used products.

关键词： single-atom catalysis hydrogenation fragrance household product coronavirus disease 2019(COVID-19)

锐钛矿型TiO_(2)负载Ni单原子用于催化丙烷脱氢

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Chinese Journal of Catalysis 2024年第2期57卷 105-113页

作者：张倩江训柱苏杨赵阳乔波涛中国科学院大连化学物理研究所中国科学院应用催化科技重点实验室辽宁大连116023 中国科学院大学北京100049 中国科学院大连化学物理研究所大连洁净能源国家实验室辽宁大连116023

丙烯市场需求日益增长,丙烷脱氢(PDH)被认为是最有前途的丙烯定向生产技术之一.作为PDH商业催化剂,贵金属Pt的高成本和CrO_(x)基催化剂的毒性使它们的发展受到限制.镍基催化剂因具有廉价、环保的特点,在多种催化反应的应用中引起了研究... 详细信息

丙烯市场需求日益增长,丙烷脱氢(PDH)被认为是最有前途的丙烯定向生产技术之一.作为PDH商业催化剂,贵金属Pt的高成本和CrO_(x)基催化剂的毒性使它们的发展受到限制.镍基催化剂因具有廉价、环保的特点,在多种催化反应的应用中引起了研究人员的广泛关注.然而,镍在高温烷烃脱氢反应中的应用较少,目前,保持反应中镍(II)物种的稳定存在仍然是镍基PDH催化剂的主要挑战.近来,单原子催化剂(SAC)在烷烃碳氢键活化过程中表现出优异的催化性能,具有较好的丙烯选择性和出色的稳定性.当镍以单个原子的形式分散在载体上时,它更有可能以带正电的状态存在,但金属单原子的稳定存在是具有挑战性的.本文以锐钛矿型的二氧化钛为载体,采用等体积浸渍法分别制备了0.05 wt%载量的单个原子分散的催化剂(Ni SAC,Ni_(1)/A-TiO_(2))和5 wt%载量的纳米颗粒(NP)催化剂(Ni_(NP)/A-TiO_(2)).结合球差电镜、原位漫反射傅里叶变换红外光谱和X射线吸收光谱等表征结果表明,Ni SAC催化剂主要含有单个Ni原子,以Ni(II)价态孤立地分散在载体上,而Ni_(NP)/A-TiO_(2)催化剂中的Ni物种主要以纳米粒子(1±0.2 nm)的形式存在.在580℃的PDH反应中,Ni_(1)/A-TiO_(2)催化剂表现出较好的本征活性和丙烯选择性,而且比相应的Ni NPs催化剂具有更好的抗积炭稳定性,在Ni_(1)/A-TiO_(2)上得到的丙烯产率约为1.96 molC_(3)H_(6)gNi^(-1)h^(-1),超过NiNP/A-TiO_(2)样品(0.03 molC_(3)H_(6)gNi^(-1)h^(-1))的65倍,Ni SAC催化剂的丙烯时空收率(STYC_(3)H_(6))约为0.2 kg h^(-1) kg_(cat)^(-1),与文献报道的大部分非贵金属催化剂STY值相当(0.02-0.3 kg h^(-1) kg_(cat)^(-1)).还原后的TiO_(2)载体因具有丰富的氧空位(OVs)和配位不饱和的Ti^(3+)表现出一定的活性,而Ni SAC得到了更高的丙烷转化率,但Ni单原子的引入并没有增加OVs和Ti^(3+)的浓度,Ni单原子催化剂的活化能低于纯载体,说明两者的活性位不同.此外,在还原条件下,由于Ni NPs与TiO_(2)载体之间的强相互作用,Ni NPs位点被TiO_(x)覆盖层(~2 nm)包裹,从而显示出较差的反应活性.综上所述,本文报道了Ni单原子催化剂在丙烷直接脱氢反应中比相应的Ni NP催化剂表现出更好的反应性能,体现了具有孤立活性位点的单原子催化剂在丙烷脱氢反应中的优势,为今后探究可用于丙烷脱氢反应的单原子催化剂的制备和应用提供参考.

关键词：丙烷脱氢单原子催化剂原子利用率丙烯选择性稳定性

Atom-by-atom fabrication of metal clusters for efficient selective hydrogenation

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Science China Chemistry 2022年第2期65卷 202-203页

作者： Yalin Guo botao qiao CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

Supported metal catalysts,in which the metal is usually finely dispersed into nanoparticles(NPs)in size of a few nanometers on high-surface-area materials,are the workhorses in heterogeneous catalysis and have been extensively used in various key industrial processes[1].However,the surface heterogeneity arising from the uneven size distribution as well as the lower atomic efficiency derived from the presence of unexposed interior atoms of metal NPs often leads to inferior activity/selectivity.

关键词： hydrogenation interior catalysis

Pd single-atom catalysts derived from strong metal-support interaction for selective hydrogenation of acetylene

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Nano Research 2022年第12期15卷 10037-10043页

作者： Yalin Guo Yangyang Li Xiaorui Du Lin Li Qike Jiang botao qiao CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China University of Chinese Academy of Sciences Beijing100049China Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou510640China Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China

Selective hydrogenation of acetylene in excess ethylene is an important reaction in both fundamental study and practical ***-based catalysts with high intrinsic activity are commonly employed,but usually suffer from low *** single-atom catalysts(SACs)usually exhibit outstanding ethylene selectivity due to the weakπ-bonding ethylene ***,the preparation of high-loading and stable Pd SACs is still confronted with a great *** this work,we report a simple strategy to fabricate Pd SACs by means of reducing conventional supported Pd catalysts at suitable temperatures to selectively encapsulate the co-existed Pd nanoparticles(NPs)/*** is based on our new finding that single atoms only manifest strong metal-support interaction(SMSI)at higher reduction temperature than that of NPs/*** derived Pd SACs(Pd1/CeO2 and Pd1/a-Fe2O3)were applied to acetylene selective hydrogenation,exhibiting much improved ethylene selectivity and high *** work offers a promising way to develop stable Pd SACs easily.

关键词： selective hydrogenation of acetylene Pd single-atom catalysts(SACs) weakπ-bonding ethylene adsorption strong metal-support interaction(SMSI)

Selective and stable Au-Cu bimetallic catalyst for CO-PROX

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Nano Research 2023年第7期16卷 9031-9038页

作者： Feng Hong Guanjian Cheng Weihao Hu Shengyang Wang Qike Jiang Junhong Fu botao qiao Jiahui Huang Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China College of Energy Soochow Institute for Energy and Materials Innovations(SIEMIS)Soochow UniversitySuzhou 215006China CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China School of Chemistry and Chemical Engineering Yulin UniversityYulin 719000China University of Chinese Academy of Sciences Beijing 100049China

Gold-based catalysts are promising in CO preferential oxidation(CO-PROX)reaction in H_(2)-rich stream on account of their high intrinsic activity for CO elimination even at ambient ***,the decrease of CO conversion at elevated temperature due to the competition of H_(2)oxidation,together with the low stability of gold nanoparticles,has posed a dear ***,we report that Au-Cu bimetallic catalyst prepared by galvanic replacement method shows a wide temperature window for CO total conversion(30-100℃)and very good catalyst stability without deactivation in a 200-h *** characterizations combined with density functional theory(DFT)calculation reveal that the synergistic effect of Au-Cu,the electron transfer from Au to Cu,leads to not only strengthened chemisorption of CO but also weakened dissociation of H_(2),both of which are helpful in inhibiting the competition of H_(2)oxidation thus widening the temperature window for CO total conversion.

关键词： gold catalysis CO preferential oxidation(CO-PROX) electronic interaction galvanic replacement

“自上而下”构筑TiO_(2)与Pt纳米簇之间的活性界面I:再分散过程和机制

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Chinese Journal of Catalysis 2024年第3期58卷 237-246页

作者：杜晓蕊黄一珂潘晓丽江训柱苏杨杨静怡郭亚琳韩冰文承彦王晨光乔波涛中国科学院大连化学物理研究所中国科学院应用催化科技重点实验室辽宁大连116023 中国科学院广州能源研究所广东广州510640 北京科学智能研究院北京100000 中国科学院大学北京100049 重庆大学化学化工学院多尺度多孔材料研究中心重庆400044 中国石化大连石油化工研究院辽宁大连116023 中国科学院可再生能源重点实验室广东广州510640

负载型金属催化剂广泛应用于现代化学化工过程,其中,金属颗粒的尺寸通常对催化性能起着至关重要的作用.尤其是,那些粒径低于2 nm的高分散金属纳米簇,不仅具有接近单原子催化剂的原子利用效率,而且展现出协同活化底物的能力.这使得它们... 详细信息

负载型金属催化剂广泛应用于现代化学化工过程,其中,金属颗粒的尺寸通常对催化性能起着至关重要的作用.尤其是,那些粒径低于2 nm的高分散金属纳米簇,不仅具有接近单原子催化剂的原子利用效率,而且展现出协同活化底物的能力.这使得它们在特定反应中能够兼具单原子和纳米催化剂的优势,并逐渐受到关注.然而,制备高稳定负载型纳米簇催化剂仍然是一项挑战.传统的“自下而上”制备策略存在成本高、产率低以及复杂配体难以去除等问题.近年来,通过“自上而下”的方法将金属纳米颗粒等聚集体再分散为单原子已经成为一种较普遍的单原子催化剂制备方法,但利用类似策略合成纳米簇催化剂的报道较少.本文通过对TiO_(2)负载的铂纳米颗粒或PtO_(2)粉末进行简单的煅烧,成功制备了高分散且热稳定的铂纳米簇,并通过系统表征和密度泛函理论(DFT)模拟深入研究了这一再分散过程和机制.首先,使用胶体沉淀法合成了TiO_(2)负载的铂纳米颗粒催化剂.在400°C空气中焙烧除去除保护剂后,铂纳米颗粒平均粒径为3.4 nm.然而,当焙烧温度升高至550°C时,Pt纳米颗粒消失,转化为高度分散的纳米簇,平均粒径约为1 nm.X射线光电子能谱和X射线吸收近边结构结果表明,再分散后铂的价态从金属态转变为+4价为主的氧化态;扩展X射线吸收精细结构的拟合结果进一步证实了再分散后铂的高价态和小尺寸.值得注意的是,与大部分金属再分散均形成单原子分散物种不同,本工作中铂在TiO_(2)载体上的再分散以纳米簇为最终物种.为了解释纳米簇的形成,详细研究了金属再分散过程.通过对照试验,排除了表面活性剂的作用,并证实形成氧化铂物种在再分散过程中起关键作用.通过DFT计算评估了可能的氧化铂中间体的化学势,结果表明铂的氧化单体,尤其是Pt_(1)(O_(2))/r110和气态PtO_(2)(g),具有更低的化学势,使得纳米颗粒的分解更有可能发生.进一步通过DFT模拟排除了以Pt_(1)(O_(2))/r110为中间体的表面扩散机理,并指出对于气相捕获机制,PtO_(2)(g)是最可能的气态中间体.模拟结果表明,PtO_(2)(g)分子优先被VTi_(5)c空位捕获并形成P_(tion)-r110位点;该位点可诱导更多的PtO_(2)(g)单体在其上聚集,从而生长为纳米簇;在550°C下焙烧时,其尺寸稳定分布在1 nm左右.综上,本工作提出一种“自上而下”的制备策略,通过金属颗粒在载体表面的再分散过程,成功合成了负载纳米簇催化剂.该制备方法简单可行,易于放大,为实现宏量制备提供了有效途径.同时,深入研究了再分散过程,揭示了纳米簇物种形成的原因和机理,为金属再分散现象提供了新的理解和认识.

关键词：多相催化纳米簇再分散金属-氧化物界面一氧化碳氧化

Ultrastable single-atom gold catalysts with strong covalent metal-support interaction （CMSI）

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Nano Research 2015年第9期8卷 2913-2924页

作者： botao qiao Jin-Xia Liang Aiqin Wang Cong-qiao Xu Jun Li Tao Zhang Jingyue (Jimmy) Liu Department of Physics Arizona State University Tempe Arizona 85287 USA State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China Department of Chemistry & Key Laboratory of Organic Optoelectronics and Molecular Engineering of the Ministry of Education Tsinghua University Beijing 100084 China Guizhou Provincial Key Laboratory of Computational Nano-Material Science Guizhou Normal College Guiyang 550018 China

Supported noble metal nanoparticles （including nanoclusters） are widely used in many industrial catalytic processes. While the finely dispersed nanostructures are highly active, they are usually thermodynamically unstable and tend to aggregate or sinter at elevated temperatures. This scenario is particularly true for supported nanogold catalysts because the gold nanostructures are easily sintered at high temperatures, under reaction conditions, or even during storage at ambient temperature. Here, we demonstrate that isolated Au single atoms dispersed on iron oxide nanocrystallites （Aul/FeOx） are much more sintering- resistant than Au nanostructures, and exhibit extremely high reaction stability for CO oxidation in a wide temperature range. Theoretical studies revealed that the positively charged and surface-anchored Aul atoms with high valent states formed significant covalent metal-support interactions （CMSIs）, thus providing the ultra-stability and remarkable catalytic performance. This work may provide insights and a new avenue for fabricating supported Au catalysts with ultra-high stability.

关键词： single-atom catalysis,goId catalyst,CO oxidation,covalent metal-supportinteraction

Highly active and sintering-resistant heteroepitaxy of Au nanoparticles on ZnO nanowires for CO oxidation

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Journal of Energy Chemistry 2016年第3期25卷 361-370页

作者： Jiaxin Liu botao qiao Yian Song Hailian Tang Yudong Huang Jingyue(Jimmy) Liu College of Chemical Engineering and Technology Harbin Institute of Technology Department of Physics Arizona State University State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Gold was supported on commercial ZnO powders(P) and homemade ZnO nanowires(NWs) by a modified deposition–precipitation method. X-ray diffraction and transmission electron microscopy investigation indicated that the size of the Au nanoparticles(NPs) depended strongly on the calcination *** Au NPs were highly dispersed( 400 °C. Such unique anchoring mechanism accounts for the much better experimentally observed sintering resistance. X-ray photoelectron spectra showed that Au existed as both metallic Au0 and Auδ+species in all the synthesized catalysts with or without calcination treatment; the ratios of Auδ+/Au0,however, varied, depending on the treatment conditions. Catalytic tests showed that the activity for CO oxidation strongly depended on the size of the Au NPs. After calcination at 600 °C, the specific rate for CO oxidation at room temperature decreased about 30 times on Au/ZnO P but only about 4 times on Au/ZnO NW. Stability tests demonstrated that the Au/ZnO NW catalysts had better stability for CO oxidation.

关键词： Gold ZnO Nanowires Epitaxy CO oxidation Sintering Stability

Enhanced stability of Pt/Al_(2)O_(3) modified by Zn promoter for catalytic dehydrogenation of ethane

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Journal of Energy Chemistry 2020年第12期29卷 14-20页

作者： Xiaoyu Li Yanliang Zhou botao qiao Xiaoli Pan Chaojie Wang Liru Cao Lin Li Jian Lin Xiaodong Wang CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Catalytic ethane dehydrogenation(EDH) to ethylene over Pt-based catalysts has received increasing interests in recent years as it is a potential alternative route to conventional steam cracking. However, the catalysts used in this reaction often suffer from rapid deactivation due to serious coke deposition and metal sintering. Herein, we reported the effects of Zn modification on the stability of Pt/Al2 O3 for *** Zn-modified sample(PtZn2/Al2 O3) exhibits stable ethane conversion(20%) with over 95% ethylene selectivity. More importantly, it exhibits a significantly low deactivation rate of only 0.003 h-1 at 600 °C for70 h, which surpasses most of previously reported catalysts. Detailed characterizations including in situ FT-IR, ethylene adsorption microcalorimetry, and HAADF-STEM etc. reveal that Zn modifier reduces the number of Lewis acid sites on the catalyst surface. Moreover, it could modify Pt sites and preferentially cover the step sites, which decrease surface energy and retard the sintering of Pt particle, then prohibiting the further dehydrogenation of ethylene to ethylidyne. Consequently, the good stability is realized due to anti-sintering and the decrease of coke formation on the Pt Zn2/Al2 O3 catalyst.

关键词： Catalytic dehydrogenation of ethane Stability PtZn/Al2O3 Zn promoter Coke